Non-Bonding Interaction of Neighboring Fe and Ni Single-Atom Pairs on MOF-Derived N-Doped Carbon for Enhanced CO2 Electroreduction,Journal of the American Chemical Society

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Non-Bonding Interaction of Neighboring Fe and Ni Single-Atom Pairs on MOF-Derived N-Doped Carbon for Enhanced CO2 Electroreduction
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2021-11-15 , DOI: 10.1021/jacs.1c08050
Long Jiao ₁ , Juntong Zhu ₂ , Yan Zhang ₁ , Weijie Yang ₃ , Siyuan Zhou ₂ , Aowen Li ₂ , Chenfan Xie ₁ , Xusheng Zheng ₄ , Wu Zhou _{2,

5} , Shu-Hong Yu ₁ , Hai-Long Jiang ₁

Affiliation

Single-atom catalysts (SACs), featuring high atom utilization, have captured widespread interests in diverse applications. However, the single-atom sites in SACs are generally recognized as independent units and the interplay of adjacent sites is largely overlooked. Herein, by the direct pyrolysis of MOFs assembled with Fe and Ni-doped ZnO nanoparticles, a novel Fe₁–Ni₁–N–C catalyst, with neighboring Fe and Ni single-atom pairs decorated on nitrogen-doped carbon support, has been precisely constructed. Thanks to the synergism of neighboring Fe and Ni single-atom pairs, Fe₁–Ni₁–N–C presents significantly boosted performances for electrocatalytic reduction of CO₂, far surpassing Fe₁–N–C and Ni₁–N–C with separate Fe or Ni single atoms. Additionally, the Fe₁–Ni₁–N–C also exhibits superior performance with excellent CO selectivity and durability in Zn-CO₂ battery. Theoretical simulations reveal that, in Fe₁–Ni₁–N–C, single Fe atoms can be highly activated by adjacent single-atom Ni via non-bonding interaction, significantly facilitating the formation of COOH* intermediate and thereby accelerating the overall CO₂ reduction. This work supplies a general strategy to construct single-atom catalysts containing multiple metal species and reveals the vital importance of the communitive effect between adjacent single atoms toward improved catalysis.

中文翻译：

相邻 Fe 和 Ni 单原子对在 MOF 衍生的 N 掺杂碳上的非键相互作用增强 CO2 电还原

具有高原子利用率的单原子催化剂（SAC）在各种应用中引起了广泛的兴趣。然而，SAC 中的单原子位点通常被认为是独立的单元，而在很大程度上忽略了相邻位点的相互作用。在此，通过由 Fe 和 Ni 掺杂的 ZnO 纳米粒子组装的 MOF 的直接热解，一种新型的 Fe ₁ -Ni ₁ -N-C 催化剂，在氮掺杂的碳载体上装饰有相邻的 Fe 和 Ni 单原子对，已经精确构建。由于相邻的 Fe 和 Ni 单原子对的协同作用，Fe ₁ –Ni ₁ –N–C 对 CO _{2 的}电催化还原性能显着提高，远远超过 Fe ₁–N–C 和 Ni ₁ –N–C 具有单独的 Fe 或 Ni 单原子。此外，Fe ₁ –Ni ₁ –N–C 在 Zn-CO ₂电池中也表现出优异的性能，具有出色的 CO 选择性和耐久性。理论模拟表明，在 Fe ₁ -Ni ₁ -N-C 中，单个 Fe 原子可以通过非键相互作用被相邻的单原子 Ni 高度活化，显着促进 COOH* 中间体的形成，从而加速整体 CO ₂减少。这项工作提供了构建包含多种金属物种的单原子催化剂的一般策略，并揭示了相邻单原子之间的共生效应对改善催化作用的重要性。

更新日期：2021-11-24

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